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首页> 外文期刊>Chemistry: A European journal >Testing electron transfer within molecular associates built around anionic C-60 and C-70 dendrofullerenes and a cationic zinc porphyrin
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Testing electron transfer within molecular associates built around anionic C-60 and C-70 dendrofullerenes and a cationic zinc porphyrin

机译：测试围绕阴离子C-60和C-70树枝状富勒烯和阳离子锌卟啉构建的分子缔合体中的电子转移

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摘要

Mono- and bis-functionalized C-60 and C-70 fullerene derivatives (DF, 1-10) that carry one or two oligoanionic dendritic termini in their malonate addends and an oligocationic octapyridinium zinc porphyrin salt (ZnP) were found to self-assemble in buffered aqueous solution to yield a novel series of 1:1 and/or 1:2 electron transfer hybrid associates. Remarkably high association constants-typically on the order of 10(8) M-1-were derived that corroborate stable complex formations. A combination of electrostatic and charge-transfer interactions that are operative between the electron-accepting DF and the electron-donating ZnP is considered to contribute to the uniquely high complex stability. First insight into intracomplex excited state interactions came from steady-state and time-resolved fluorescence quenching experiments that were performed with the molecular ZnP/DF hybrid associates. Excited state quenching processes are, for example, evident in form of a bi-exponential fluorescence decay of ZnP-corresponding to a distribution of associated and non-associated ZnP. Unambiguous evidence for an intracomplex electron transfer quenching, namely, formation of ZnP center dot+/C-60(center dot-) and ZnP center dot+/C-70(center dot-) radical ion pairs, was gathered in time-resolved transient absorption measurements. Lifetimes of these radical ion-pairs range from nanoseconds to a few microseconds.
机译：发现单官能团和双官能团的C-60和C-70富勒烯衍生物（DF，1-10）在其丙二酸酯加成物中带有一个或两个低聚阴离子树突状末端和一个低聚八吡啶吡啶鎓锌卟啉盐（ZnP）自组装在缓冲的水溶液中产生一系列新的1：1和/或1：2电子转移杂合体。得出了很高的缔合常数，通常约为10（8）M-1，可证实稳定的络合物形成。在电子接受的DF和电子提供的ZnP之间起作用的静电和电荷转移相互作用的组合被认为有助于独特的高络合物稳定性。对内复合物激发态相互作用的初步了解来自使用分子ZnP / DF杂化分子进行的稳态和时间分辨的荧光猝灭实验。激发态猝灭过程例如以ZnP的双指数荧光衰减形式出现，这与缔合和非缔合ZnP的分布相对应。在时间分辨的瞬态吸收中收集了复杂的电子转移猝灭的明确证据，即形成ZnP中心点+ / C-60（中心点-）和ZnP中心点+ / C-70（中心点-）自由基离子对。测量。这些自由基离子对的寿命范围从纳秒到几微秒。

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